A. Rap

Large contribution of natural aerosols to uncertainty in indirect forcing.

The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

Ion-induced nucleation of pure biogenic particles

Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

Global atmospheric particle formation from CERN CLOUD measurements

Observations made in the CLOUD chamber at CERN illuminate atmospheric particle formation. How new particles form New particle formation in the atmosphere produces around half of the cloud condensation nuclei that seed cloud droplets. Such particles have a pivotal role in determining the properties of clouds and the global radiation balance. Dunne et al. used the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN to construct a model of aerosol formation based on laboratory-measured nucleation rates. They found that nearly all nucleation involves either ammonia or biogenic organic compounds. Furthermore, in the present-day atmosphere, cosmic ray intensity cannot meaningfully affect climate via nucleation. Science, this issue p. 1119 Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. We built a global model of aerosol formation by using extensive laboratory measurements of rates of nucleation involving sulfuric acid, ammonia, ions, and organic compounds conducted in the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds, in addition to sulfuric acid. A considerable fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied, variations in cosmic ray intensity do not appreciably affect climate through nucleation in the present-day atmosphere.

Parameterization of contrails in the UK Met Office Climate Model

Persistent contrails are believed to currently have a relatively small but significant positive radiative forcing on climate. With air travel predicted to continue its rapid growth over the coming years, the contrail warming effect on climate is expected to increase. Nevertheless, there remains a high level of uncertainty in the current estimates of contrail radiative forcing. Contrail formation depends mostly on the aircraft flying in cold and moist enough air masses. Most studies to date have relied on simple parameterizations using averaged meteorological conditions. In this paper we take into account the short-term variability in background cloudiness by developing an on-line contrail parameterization for the UK Met Office climate model. With this parameterization, we estimate that for the air traffic of year 2002 the global mean annual linear contrail coverage was approximately 0.11%. Assuming a global mean contrail optical depth of 0.2 or smaller and assuming hexagonal ice crystals, the corresponding contrail radiative forcing was calculated to be less than 10 mW m(-2) in all-sky conditions. We find that the natural cloud masking effect on contrails may be significantly higher than previously believed. This new result is explained by the fact that contrails seem to preferentially form in cloudy conditions, which ameliorates their overall climate impact by approximately 40%.

A case study of the radiative forcing of persistent contrails evolving into contrail-induced cirrus

over 50,000 km 2 . The shortwave (SW) and longwave (LW) radiative forcing of the contrail-induced cirrus is estimated using a combination of geostationary satellite instruments, numerical weather prediction models, and surface observation sites. As expected, the net radiative effect is a relatively small residual of the much stronger but opposing SW and LW effects, locally totaling around 10 W m �2 during daylight hours and 30 W m �2 during nighttime. A simple estimate indicates that this single localized event may have generated a global-mean radiative forcing of around 7% of recent estimates of the persistent contrail radiative forcing due to the entire global aircraft fleet on a diurnally averaged basis. A single aircraft operating in conditions favorable for persistent contrail formation appears to exert a contrail-induced radiative forcing some 5000 times greater (in W m � 2 km �1 ) than recent estimates of the average persistent contrail radiative forcing from the entire civil aviation fleet. This study emphasizes the need to establish whether similar events are common or highly unusual for a confident assessment of the total climate effect of aviation to be made.

Intercomparison of radiative forcing calculations of stratospheric water vapour and contrails

Seven groups have participated in an intercomparison study of calculations of radiative forcing (RF) due to stratospheric water vapour (SWV) and contrails. A combination of detailed radiative transfer schemes and codes for global-scale calculations have been used, as well as a combination of idealized simulations and more realistic global-scale changes in stratospheric water vapour and contrails. Detailed line-by-line codes agree within about 15 % for longwave (LW) and shortwave (SW) RF, except in one case where the difference is 30 %. Since the LW and SW RF due to contrails and SWV changes are of opposite sign, the differences between the models seen in the individual LW and SW components can be either compensated or strengthened in the net RF, and thus in relative terms uncertainties are much larger for the net RF. Some of the models used for global-scale simulations of changes in SWV and contrails differ substantially in RF from the more detailed radiative transfer schemes. For the global-scale calculations we use a method of weighting the results to calculate a best estimate based on their performance compared to the more detailed radiative transfer schemes in the idealized simulations.

Fires increase Amazon forest productivity through increases in diffuse radiation

Atmospheric aerosol scatters solar radiation increasing the fraction of diffuse radiation and the efficiency of photosynthesis. We quantify the impacts of biomass burning aerosol (BBA) on diffuse radiation and plant photosynthesis across Amazonia during 1998–2007. Evaluation against observed aerosol optical depth allows us to provide lower and upper BBA emissions estimates. BBA increases Amazon basin annual mean diffuse radiation by 3.4–6.8% and net primary production (NPP) by 1.4–2.8%, with quoted ranges driven by uncertainty in BBA emissions. The enhancement of Amazon basin NPP by 78–156 Tg C a−1 is equivalent to 33–65% of the annual regional carbon emissions from biomass burning. This NPP increase occurs during the dry season and acts to counteract some of the observed effect of drought on tropical production. We estimate that 30–60 Tg C a−1 of this NPP enhancement is within woody tissue, accounting for 8–16% of the observed carbon sink across mature Amazonian forests.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

Significance A mechanism for the formation of atmospheric aerosols via the gas to particle conversion of highly oxidized organic molecules is found to be the dominant aerosol formation process in the preindustrial boundary layer over land. The inclusion of this process in a global aerosol model raises baseline preindustrial aerosol concentrations and could lead to a reduction of 27% in estimates of anthropogenic aerosol radiative forcing. The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol–cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20–100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m−2 (27%) to −0.60 W m−2. Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Uncertainty in the magnitude of aerosol-cloud radiative forcing over recent decades

Aerosols and their effect on the radiative properties of clouds are one of the largest sources of uncertainty in calculations of the Earths energy budget. Here the sensitivity of aerosol-cloud albedo effect forcing to 31 aerosol parameters is quantified. Sensitivities are compared over three periods; 1850-2008, 1978-2008, and 1998-2008. Despite declining global anthropogenic SO2 emissions during 1978-2008, a cancelation of regional positive and negative forcings leads to a near-zero global mean cloud albedo effect forcing. In contrast to existing negative estimates, our results suggest that the aerosol-cloud albedo effect was likely positive (0.006 to 0.028 W m −2 ) in the recent decade, making it harder to explain the temperature hiatus as a forced response. Proportional contributions to forcing variance from aerosol processes and natural and anthropogenic emissions are found to be period dependent. To better constrain forcing estimates, the processes that dominate uncertainty on the timescale of interest must be better understood.

Extending water vapor trend observations over Boulder into the tropopause region: Trend uncertainties and resulting radiative forcing

Thirty years of balloon-borne measurements over Boulder (40°N, 105°W) are used to investigate the water vapor trend in the tropopause region. This analysis extends previously published trends, usually focusing on altitudes greater than 16 km, to lower altitudes. Two new concepts are applied: (1) Trends are presented in a thermal tropopause (TP) relative coordinate system from -2 km below to 10 km above the TP, and (2) sonde profiles are selected according to TP height. Tropical (TP z > 14 km), extratropical (TP z < 12 km), and transitional air mass types (12 km < TP z < 14 km) reveal three different water vapor reservoirs. The analysis based on these concepts reduces the dynamically induced water vapor variability at the TP and principally favors refined water vapor trend studies in the upper troposphere and lower stratosphere. Nonetheless, this study shows how uncertain trends are at altitudes -2 to +4 km around the TP. This uncertainty in turn has an influence on the uncertainty and interpretation of water vapor radiative effects at the TP, which are locally estimated for the 30 year period to be of uncertain sign. The much discussed decrease in water vapor at the beginning of 2001 is not detectable between -2 and 2 km around the TP. On lower stratospheric isentropes, the water vapor change at the beginning of 2001 is more intense for extratropical than for tropical air mass types. This suggests a possible link with changing dynamics above the jet stream such as changes in the shallow branch of the Brewer-Dobson circulation.